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MEL-type Pure-Silica Zeolite Nanocrystals Prepared by an Evaporation-Assisted Two-Stage Synthesis Method as Ultra-Low-k Materials

机译:蒸发辅助两阶段合成法制备的MEL型纯硅沸石纳米晶为超低k材料

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摘要

A MEL-type pure-silica zeolite (PSZ), prepared by spin-on of nanoparticle suspensions, has been shown to be a promising ultra-low-dielectric-constant (k) material because of its high mechanical strength, hydrophobicity, and chemical stability. In our previous works, a two-stage synthesis method was used to synthesize a MEL-zeolite nanoparticle suspension, in which both nanocrystal yield and particle size of the zeolite suspension increased with increasing synthesis time. For instance, at a crystal yield of 63%, the particle size is 80 nm, which has proved to be too large because it introduces a number of problems for the spin-on films, including large surface roughness, surface striations, and large mesopores. In the current study, the two-stage synthesis method is modified into an evaporation-assisted two-stage method by adding a solvent-evaporation process between the two thermal-treatment steps. The modified method can yield much smaller particle sizes (e.g., 14vs. 80 nm) while maintaining the same nanocrystal yields as the two-stage synthesis. Furthermore, the nanoparticle suspensions from the evaporation-assisted two-stage synthesis show a bimodal particle size distribution. The primary nanoparticles are around 14nm in size and are stable in the final suspension with 60% solvent evaporation. The factors that affect nanocrystal synthesis are discussed, including the concentration, pH value, and viscosity. Spin-on films prepared by using suspensions synthesized this way have no striations and improved elastic modulus (9.67 ± 1.48 GPa vs. 7.82 ± 1.30 GPa), as well as a similar k value (1.91 ±0.09 vs. 1.89 ±0.08) to the previous two-stage synthesized films.
机译:通过旋涂纳米颗粒悬浮液制备的MEL型纯硅沸石(PSZ)由于其高机械强度,疏水性和化学性质而被证明是一种有前途的超低介电常数(k)材料。稳定性。在我们以前的工作中,采用两步合成法合成MEL沸石纳米颗粒悬浮液,其中纳米晶体的产率和沸石悬浮液的粒径均随合成时间的增加而增加。例如,在晶体产率为63%时,粒径为80 nm,这已被证明太大,因为它给旋涂膜带来了许多问题,包括大的表面粗糙度,表面条纹和大的中孔。在当前的研究中,通过在两个热处理步骤之间添加溶剂蒸发过程,将两步合成方法修改为蒸发辅助两步方法。改进的方法可以产生小得多的粒径(例如14vs.80nm),同时保持与两步合成相同的纳米晶体产率。此外,来自蒸发辅助两步合成的纳米颗粒悬浮液显示出双峰粒度分布。初级纳米粒子的尺寸约为14nm,在最终悬浮液中稳定,溶剂蒸发60%。讨论了影响纳米晶体合成的因素,包括浓度,pH值和粘度。使用这种方法合成的悬浮液制备的旋涂膜没有条纹,并且弹性模量有所提高(9.67±1.48 GPa与7.82±1.30 GPa),并且k值(1.91±0.09与1.89±0.08)相似。以前的两阶段合成电影。

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